Prospective Cohort Study

Metal–organic frameworks (MOFs) display a wide range of luminescent behaviors resulting from the multifaceted nature of their structure. In this critical review we discuss the origins of MOF luminosity, which include the linker, the coordinated metal ions, antenna effects, excimer and exciplex formation, and guest molecules. The literature describing these effects is comprehensively surveyed, including a categorization of each report according to the type of luminescence observed. Finally, we discuss potential applications of luminescent MOFs. This review will be of interest to researchers and synthetic chemists attempting to design luminescent MOFs, and those engaged in the extension of MOFs to applications such as chemical, biological, and radiation detection, medical imaging, and electro-optical devices (141 references).

Luminescent Metal–Organic Frameworks

Intestinal microbiota metabolism of choline and phosphatidylcholine produces trimethylamine (TMA), which is further metabolized to a proatherogenic species, trimethylamine-N-oxide (TMAO). We demonstrate here that metabolism by intestinal microbiota of dietary L-carnitine, a trimethylamine abundant in red meat, also produces TMAO and accelerates atherosclerosis in mice. Omnivorous human subjects produced more TMAO than did vegans or vegetarians following ingestion of L-carnitine through a microbiota-dependent mechanism. The presence of specific bacterial taxa in human feces was associated with both plasma TMAO concentration and dietary status. Plasma L-carnitine levels in subjects undergoing cardiac evaluation (n = 2,595) predicted increased risks for both prevalent cardiovascular disease (CVD) and incident major adverse cardiac events (myocardial infarction, stroke or death), but only among subjects with concurrently high TMAO levels. Chronic dietary L-carnitine supplementation in mice altered cecal microbial composition, markedly enhanced synthesis of TMA and TMAO, and increased atherosclerosis, but this did not occur if intestinal microbiota was concurrently suppressed. In mice with an intact intestinal microbiota, dietary supplementation with TMAO or either carnitine or choline reduced in vivo reverse cholesterol transport. Intestinal microbiota may thus contribute to the well-established link between high levels of red meat consumption and CVD risk.

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Intestinal microbiota metabolism of L-carnitine, a nutrient in red meat, promotes atherosclerosis

Metal–organic frameworks (MOFs), a class of hybrid materials formed by the self-assembly of polydentate bridging ligands and metal-connecting points, have been studied for a variety of applications. Recently, these materials have been scaled down to nanometer sizes, and this Account details the development of nanoscale metal–organic frameworks (NMOFs) for biomedical applications. NMOFs possess several potential advantages over conventional nanomedicines such as their structural and chemical diversity, their high loading capacity, and their intrinsic biodegradability. Under relatively mild conditions, NMOFs can be obtained as either crystalline or amorphous materials. The particle composition, size, and morphology can be easily tuned to optimize the final particle properties. Researchers have employed two general strategies to deliver active agents using NMOFs: by incorporating active agents into the frameworks or by loading active agents into the pores and channels of the NMOFs. The modification of NMOF s...

/pdf/nanoscale-metal-organic-frameworks-for-biomedical-imaging-fwvtz1u39w.pdf

Nanoscale Metal–Organic Frameworks for Biomedical Imaging and Drug Delivery

Solar energy is an alternative, sustainable energy source for mankind. Finding a convenient way to convert sunlight energy into chemical energy is a key step towards realizing large-scale solar energy utilization. Owing to their structural regularity and synthetic tunability, metal–organic frameworks (MOFs) provide an interesting platform to hierarchically organize light-harvesting antennae and catalytic centers to achieve solar energy conversion. Such photo-driven catalytic processes not only play a critical role in the solar to chemical energy conversion scheme, but also provide a novel methodology for the synthesis of fine chemicals. In this review, we summarize the fundamental principles of energy transfer and photocatalysis and provide an overview of the latest progress in energy transfer, light-harvesting, photocatalytic proton and CO2 reduction, and water oxidation using MOFs. The applications of MOFs in organic photocatalysis and degradation of model organic pollutants are also discussed.

Metal–organic frameworks for artificial photosynthesis and photocatalysis

The fabrication of conventional PDMS on glass lab-on-a-chip (LOC) devices, using templates printed with a commercial (2299 US$) micro-stereo lithography 3D printer, is demonstrated. Printed templates replace clean room and photolithographic fabrication resources and deliver resolutions of 50 μm, and up to 10 μm in localized hindrances, whereas the templates are smooth enough to allow direct transfer and proper sealing to glass substrates. 3D printed templates accommodate multiple thicknesses, from 50 μm up to several mm within the same template, with no additional processing cost or effort. This capability is exploited to integrate silicone tubing easily, to improve micromixer performance and to produce multilevel fluidics with simple access to independent functional surfaces, which is illustrated by time-resolved glucose detection. The templates are reusable, can be fabricated in under 20 min, with an average cost of 0.48 US$, which promotes broader access to established LOC configurations with minimal fabrication requirements, relieves LOC fabrication from design skills and provides a versatile LOC development platform.

PDMS lab-on-a-chip fabrication using 3D printed templates

Chemosensing based on angle-resolved surface plasmon resonance is demonstrated on intact cell phones using a disposable optical coupler and software to configure illumination and acquisition. This ...

Surface plasmon resonance chemical sensing on cell phones.

Ultrasmall gadolinium oxide nanoparticles doped with terbium ions were synthesized by the polyol route and characterized as a potentially bifunctional material with both fluorescent and magnetic co ...

Synthesis and Characterization of Tb3+-Doped Gd2O3 Nanocrystals : A Bifunctional Material with Combined Fluorescent Labeling and MRI Contrast Agent Properties

Versatile prototyping of 3D printed lab-on-a-chip devices, supporting different forms of sample delivery, transport, functionalization and readout, is demonstrated with a consumer grade printer, which centralizes all critical fabrication tasks. Devices cost 0.57US$ and are demonstrated in chemical sensing and micromixing examples, which exploit established principles from reference technologies.

Low cost lab-on-a-chip prototyping with a consumer grade 3D printer

We report the self-assembly of stable nanoscale coordination polymers (NCPs), which exhibit temperature-controlled guest encapsulation and release, as well as an efficient light-harvesting property. NCPs are obtained by coordination-directed organization of pi-conjugated dicarboxylate (L1) and lanthanide metal ions Gd(III), Eu(III), and Yb(III) in a DMF system. Guest molecules trans-4-styryl-1-methylpyridiniumiodide (D1) and methylene blue (D2) can be encapsulated into NCPs, and the loading amounts can be controlled by changing reaction temperatures. Small angle X-ray diffraction (SAXRD) results reveal that the self-assembled discus-like NCPs exhibit long-range ordered structures, which remain unchanged after guest encapsulations. Experimental results reveal that the negatively charged local environment around the metal connector is the driving force for the encapsulation of cationic guests. The D1 molecules encapsulated in NCPs at 140 degrees C can be released gradually at room temperature in DMF. Guest-loaded NCPs exhibit efficient light harvesting with energy transfer from the framework to the guest D1 molecule, which is studied by photoluminescence and fluorescence lifetime decays. This coordination-directed encapsulation approach is general and should be extended to the fabrication of a wide range of multifunctional nanomaterials.

Anke Suska

Papers

PDMS lab-on-a-chip fabrication using 3D printed templates

Surface plasmon resonance chemical sensing on cell phones.

Synthesis and Characterization of Tb3+-Doped Gd2O3 Nanocrystals : A Bifunctional Material with Combined Fluorescent Labeling and MRI Contrast Agent Properties

Low cost lab-on-a-chip prototyping with a consumer grade 3D printer

Nanoscale Ln(III)-carboxylate coordination polymers (Ln = Gd, Eu, Yb): temperature-controlled guest encapsulation and light harvesting